苯来石氧硫属化物 Sr2MGe2OS6（M = Mn、Zn 和 Cd）中增强的二次谐波生成效率和双折射,Chemistry of Materials

当前位置： X-MOL 学术 › Chem. Mater. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

苯来石氧硫属化物 Sr2MGe2OS6（M = Mn、Zn 和 Cd）中增强的二次谐波生成效率和双折射
Chemistry of Materials ( IF 7.2 ) Pub Date : 2022-04-07 , DOI: 10.1021/acs.chemmater.2c00385
Mao-Yin Ran _{1,

2} , Sheng-Hua Zhou _{1,

2} , Bingxuan Li ₁ , Wenbo Wei _{1,

2} , Xin-Tao Wu ₁ , Hua Lin _{1,

3} , Qi-Long Zhu _{1,

3}

Affiliation

同时调节和控制非中心对称 (NCS) 晶体的非线性二次谐波 (SHG) 系数 ( deff) 和线性双折射 (Δn )是_改善非线性光学 (NLO) 的关键方面性能，但它仍然是现代激光技术和科学的巨大挑战。在此，通过简便的部分等价化学取代策略，成功地设计和合成了一系列由硅镁石型氧化物衍生的 NCS 氧硫族化合物 Sr ₂ MGe ₂ OS ₆ (M = Mn、Zn 和 Cd)。这些同构化合物在四方 NCS 空间群P 4̅21 m中结晶_{（第 113 号）并具有由异质配体 [GeOS 3} ] 和四面体 [MS ₄ ] 不对称建筑单元 (ABU)组成的独特的二维开罗五边形平铺层。与母方硅石型氧化物相比，衍生的标题化合物不仅成功实现了相位匹配性转变[即从非相位匹配（NPM）到相位匹配（PM）]，而且大大提高了IR-NLO性能（尤其是同时提升d _eff和 Δ n）。Sr ₂ CdGe ₂ OS ₆在氧硫族化合物中表现出最好的综合性能，包括宽的 PM 截止边缘 (>525 nm)、强的d _eff（0.8 × AgGaS ₂），巨大的激光诱导损伤阈值（19.2 × AgGaS ₂），大带隙（3.62 eV），以及宽传输截止区（0.28-12.0 μm）。此外，这种mellite型结构中高度扭曲的[GeOS _{3 ] ABU被证明是有利可图的双功能NLO活性单元，有助于寻找和设计具有大}Δn和强d的新型IR-NLO晶体_效果基于实验结果和理论计算。这项工作展示了 PM 黄柱石型氧硫属化合物的第一个例子，并为通过部分等价化学取代方法的相匹配性转变提供了新的视角，这将对未来高性能 IR-NLO 杂阴离子材料的设计起到建设性的作用。

"点击查看英文标题和摘要"

Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)

Simultaneous regulation and control of non-linear second-harmonic-generation (SHG) coefficients (d_eff) and linear birefringence (Δn) of non-centrosymmetric (NCS) crystals is a crucial aspect of improving the non-linear optical (NLO) performance, yet it remains a huge challenge in modern laser techniques and science. Herein, a series of melilite-type oxide-derived NCS oxychalcogenides, Sr₂MGe₂OS₆ (M = Mn, Zn, and Cd), are successfully designed and synthesized through a facile partial isovalent chemical substitution strategy. These isostructural compounds crystallize in the tetragonal NCS space group P4̅21m (no. 113) and feature unique two-dimensional Cairo pentagonal tiling layers composed of heteroligand [GeOS₃] and tetrahedral [MS₄] asymmetric building units (ABUs). Compared to the parent melilite-type oxides, the derived title compounds not only successfully realize the phase matchability transformation [i.e., from non-phase-matching (NPM) to phase-matching (PM)] but also greatly improve the IR-NLO performance (especially, simultaneously boosting d_eff and Δn). Sr₂CdGe₂OS₆ exhibits the best comprehensive performance among oxychalcogenides, including a wide PM cutoff edge (>525 nm), a strong d_eff (0.8 × AgGaS₂), a giant laser-induced damage threshold (19.2 × AgGaS₂), a large band gap (3.62 eV), as well as a broad transmission cutoff region (0.28–12.0 μm). Furthermore, highly distorted [GeOS₃] ABU in this melilite-type structure is proved to be the profitable bifunctional NLO-active unit, which can contribute to the search and design of novel IR-NLO crystals with a large Δn and a strong d_eff based on the experimental results and theoretical calculations. This work demonstrates the first examples of PM melilite-type oxychalcogenides and offers new perspectives on the phase matchability transformation through the partial isovalent chemical substitution approach, which will play a constructive role in the future design of high-performance IR-NLO heteroanionic materials.

更新日期：2022-04-07

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南